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We report the existence of a sizeable quantum tunnelling splitting betweenthe two lowest electronic spin levels of mononuclear Ni complexes. The levelanti-crossing, or magnetic clock transition, associated with this gap has beendirectly monitored by heat capacity experiments. The comparison of theseresults with those obtained for a Co derivative, for which tunnelling isforbidden by symmetry, shows that the clock transition leads to an effectivesuppression of intermolecular spin-spin interactions. In addition, we show thatthe quantum tunnelling splitting admits a chemical tuning via the modificationof the ligand shell that determines the crystal field and the magneticanisotropy. These properties are crucial to realize model spin qubits thatcombine the necessary resilience against decoherence, a proper interfacing withother qubits and with the control circuitry and the ability to initialize themby cooling.

Chemical tuning of spin clock transitions in molecular monomers based on nuclear spin-free Ni(II)